Mechanochemical Adhesion and Plasticity in Multifiber Hydrogel Networks

Area of Science:

• Materials Science
• Biomaterials Engineering
• Polymer Chemistry

Background:

• The extracellular matrix (ECM) exhibits mechanochemical properties, adapting to mechanical loads via structural changes and altered interfiber bonding.
• Synthetic materials that replicate ECM mechanochemical properties could offer enhanced reinforcement, self-adhesion, and biomimicry.

Purpose of the Study:

• To engineer synthetic fibrous materials with force-responsive properties akin to the natural ECM.
• To develop a method for creating self-adhering and reinforcing fibrous hydrogel networks.

Main Methods:

• Electrospinning of multiple hydrogel populations containing complementary chemical moieties (aldehyde and hydrazide groups).
• Induction of covalent bonding between fibers upon mechanical loading.
• Fabrication of macroscale structures (tubes, scaffolds) from the engineered hydrogel fibers.

Main Results:

• Fiber interactions under mechanical load resulted in microscale anisotropy.
• Significant increases in material stiffness and plastic deformation were observed.
• Successful fabrication of macroscale structures while preserving microscale fibrous architecture.

Conclusions:

• Multifiber hydrogel networks with tunable mechanochemical properties were successfully developed.
• The engineered materials demonstrate reinforcement and self-adhesion under mechanical load.
• The principles for engineering plasticity are broadly applicable to various material systems and applications.